Multi-criteria analysis of strategies towards sustainable recycling of phosphorus from sewage sludge in Austria.

To promote optimal phosphorus (P) recovery from municipal wastewater and sewage sludge with viable legal instruments, it is imperative to understand the regional and national consequences of different legal requirements for recycling. In this study we develop a scenario-based analysis to assess the environmental and economic impact of different national P recovery strategies in the context of a detailed representation of the existing Austrian wastewater infrastructure. This assessment combines material flow analysis, life cycle assessment and life cycle costing and includes the indicators P recycling rate, P utilization degree, heavy metal removal rate, share of heavy metals' content in wastewater redirected to agricultural soils, global warming potential, cumulated energy demand, terrestrial acidification potential, volume of freight transport and annual costs. The following main conclusions can be drawn. P recovery from ash shows the highest potential regarding the utilization of P from wastewater. A high P utilization from wastewater should rely on recovery technologies that decontaminate products, otherwise pollutant loads to agricultural soils might increase. P recovery to the extent of 60-85 % of P in WWTPs influent can be achieved by savings/costs of -0.8 to +4.7 EUR inhabitant-1 yr-1 in addition to current cost of the wastewater treatment/sludge disposal system. Key factors to be considered for costs are the choice of recovery process, revenues from products, and the use of existing incineration infrastructure. P recovery can lead to the reduction of greenhouse gas emissions in Austria if nitrous oxide emissions from sludge incineration are limited and efficient heat utilization strategies are implemented. There is a trade-off in terms of environmental and economic costs in choosing a more centralized or decentralized mono-incineration strategy.

A source-based framework to estimate the annual load of PFAS in municipal wastewater.

Per- and Polyfluoroalkyl substances (PFAS) are a class of persistent chemicals, whose impact has been observed in various environmental compartments. Wastewater treatment plants (WWTPs) are considered a major emission pathway of PFAS, specifically in the context of the aquatic environment. The goal of this study was to develop a compartmentalized, source-based load estimation model of 7 PFAS within the municipal wastewater influent. Consumer statistics, data from literature on PFAS concentrations and release during use, and specific sampling activities for environmental flows in the related city were used to estimate per capita emission loads. Model results were compared with loads obtained through the monitoring campaign at the municipal WWTP influent. A wide range of discrepancies (≈5 % to ≈90 %) between loads observed in the WWTP influent and source based model estimates was noticed. The loads less accounted by the model were associated with sulfonic acids (PFSAs), whereas for carboxylic acids (PFCAs) most of the observed loads could be reasonably explained by the model, with even an overestimation of nearly 5 % noted for PFNA. Higher heterogeneity in sources was observed in the PFCA group, with a noticeable dominance in the share of consumer products. PFSAs had less of a consumer product input (<20 %), with the rest of the modelled load being attributed to environmental inputs. A large gap of unknown loads of PFSAs indicates a need for examination of other, not yet quantified activities that can potentially explain the remainder of the observed load. Especially commercial activities are considered as potential additional sources for PFSAs. These findings signify the importance of PFAS that originate from both consumer products, as well as environmental inputs in the overall load contribution into the sewage, while identifying the need for further investigation into commercial sources of PFAS emitted into the municipal wastewater.

Pollutant source or sink? Adsorption and mobilization of PFOS and PFOA from sediments in a large shallow lake with extended reed belt.

In this study, we i) assessed the occurrence of perfluorooctane sulfonate (PFOS) and perfluorooctanoate (PFOA) in sediments, pore water, and bulk water from three different areas in Lake Neusiedl, Austria, and ii) investigated mechanisms regulating adsorption and remobilization of these substances under different conditions via multiple lab-scale experiments. The adsorption capacity was mainly influenced by sediments' organic matter content, oxide composition, and pre-loading. Results suggest that a further increase of PFAS-concentrations in the open lake can be partly buffered by sediment transport to the littoral zone and adsorption to sediments in the extended reed belt. But, under current conditions, the conducted experiments revealed a real risk for mobilization of PFOS and PFOA from reed belt sediments that may lead to their transport back into the lake. The amount of desorbed PFAS is primarily dependent on water/sediment- or pore water/water-ratios and the concentration gradient. In contrast, water matrix characteristics and oxygen levels played a minor role in partitioning. The highest risk for remobilizing PFOS and PFOA was observed in experiments with sediments taken near the only major tributary to the lake (river Wulka), which had the highest pre-loading. The following management advice for water transport between high and low polluted areas can be derived based on the results. First, to reduce emissions into Lake waters from polluted tributaries like the Wulka river, we recommend diffuse pathways through the reed belt in the lake's littoral to reduce pollutant transport into the Lake and avoid high local sediment loadings. Second, water exchange with dried-up areas with probable higher loadings should be carefully handled and monitored to avoid critical back transport in the open lake. And third, general work in the reed belt or generally in the reed should be accompanied by monitoring to prevent uncontrolled remobilization in the future.

Setback distances between small biological wastewater treatment systems and drinking water wells against virus contamination in alluvial aquifers.

Contamination of groundwater by pathogenic viruses from small biological wastewater treatment system discharges in remote areas is a major concern. To protect drinking water wells against virus contamination, safe setback distances are required between wastewater disposal fields and water supply wells. In this study, setback distances are calculated for alluvial sand and gravel aquifers for different vadose zone and aquifer thicknesses and horizontal groundwater gradients. This study applies to individual households and small settlements (1-20 persons) in decentralized locations without access to receiving surface waters but with the legal obligation of biological wastewater treatment. The calculations are based on Monte Carlo simulations using an analytical model that couples vertical unsaturated and horizontal saturated flow with virus transport. Hydraulic conductivities and water retention curves were selected from reported distribution functions depending on the type of subsurface media. The enteric virus concentration in effluent discharge was calculated based on reported ranges of enteric virus concentration in faeces, virus infectivity, suspension factor, and virus reduction by mechanical-biological wastewater treatment. To meet the risk target of <10-4infections/person/year, a 12 log10 reduction was required, using a linear dose-response relationship for the total amount of enteric viruses, at very low exposure concentrations. The results of this study suggest that the horizontal setback distances vary widely ranging 39 to 144m in sand aquifers, 66-289m in gravel aquifers and 1-2.5km in coarse gravel aquifers. It also varies for the same aquifers, depending on the thickness of the vadose zones and the groundwater gradient. For vulnerable fast-flow alluvial aquifers like coarse gravels, the calculated setback distances were too large to achieve practically. Therefore, for this category of aquifer, a high level of treatment is recommended before the effluent is discharged to the ground surface.

Phosphorus recovery from municipal wastewater: An integrated comparative technological, environmental and economic assessment of P recovery technologies.

Phosphorus (P) is an essential and limited resource. Municipal wastewater is a promising source of P via reuse and could be used to replace P derived from phosphate rocks. The agricultural use of sewage sludge is restricted by legislation or is not practiced in several European countries due to environmental risks posed by organic micropollutants and pathogens. Several technologies have been developed in recent years to recover wastewater P. However, these technologies target different P-containing flows in wastewater treatment plants (effluent, digester supernatant, sewage sludge, and sewage sludge ash), use diverse engineering approaches and differ greatly with respect to P recycling rate, potential of removing or destroying pollutants, product quality, environmental impact and cost. This work compares 19 relevant P recovery technologies by considering their relationships with existing wastewater and sludge treatment systems. A combination of different methods, such as material flow analysis, damage units, reference soil method, annuity method, integrated cost calculation and a literature study on solubility, fertilizing effects and handling of recovered materials, is used to evaluate the different technologies with respect to technical, ecological and economic aspects. With regard to the manifold origins of data an uncertainty concept considering validity of data sources is applied. This analysis revealed that recovery from flows with dissolved P produces clean and plant-available materials. These techniques may even be beneficial from economic and technical perspectives under specific circumstances. However, the recovery rates (a maximum of 25%) relative to the wastewater treatment plant influent are relatively low. The approaches that recover P from sewage sludge apply complex technologies and generally achieve effective removal of heavy metals at moderate recovery rates (~40-50% relative to the WWTP input) and comparatively high costs. Sewage sludge ash is the most promising P source, with recovery rates of 60-90% relative to the wastewater P. The costs highly depend on the purity requirements of the recycled products but can be kept comparatively low, especially if synergies with existing industrial processes are exploited.

Occurrence of human-associated Bacteroidetes genetic source tracking markers in raw and treated wastewater of municipal and domestic origin and comparison to standard and alternative indicators of faecal pollution.

This was a detailed investigation of the seasonal occurrence, dynamics, removal and resistance of human-associated genetic Bacteroidetes faecal markers (GeBaM) compared with ISO-based standard faecal indicator bacteria (SFIB), human-specific viral faecal markers and one human-associated Bacteroidetes phage in raw and treated wastewater of municipal and domestic origin. Characteristics of the selected activated sludge wastewater treatment plants (WWTPs) from Austria and Germany were studied in detail (WWTPs, n = 13, connected populations from 3 to 49000 individuals), supported by volume-proportional automated 24-h sampling and chemical water quality analysis. GeBaM were consistently detected in high concentrations in raw (median log10 8.6 marker equivalents (ME) 100 ml(-1)) and biologically treated wastewater samples (median log10 6.2-6.5 ME 100 ml(-1)), irrespective of plant size, type and time of the season (n = 53-65). GeBaM, Escherichia coli, and enterococci concentrations revealed the same range of statistical variability for raw (multiplicative standard deviations s* = 2.3-3.0) and treated wastewater (s* = 3.7-4.5), with increased variability after treatment. Clostridium perfringens spores revealed the lowest variability for raw wastewater (s* = 1.5). In raw wastewater correlations among microbiological parameters were only detectable between GeBaM, C. perfringens and JC polyomaviruses. Statistical associations amongst microbial parameters increased during wastewater treatment. Two plants with advanced treatment were also investigated, revealing a minimum log10 5.0 (10th percentile) reduction of GeBaM in the activated sludge membrane bioreactor, but no reduction of the genetic markers during UV irradiation (254 nm). This study highlights the potential of human-associated GeBaM to complement wastewater impact monitoring based on the determination of SFIB. In addition, human-specific JC polyomaviruses and adenoviruses seem to be a valuable support if highly specific markers are needed.

Automated Sampling Procedures Supported by High Persistence of Bacterial Fecal Indicators and Bacteroidetes Genetic Microbial Source Tracking Markers in Municipal Wastewater during Short-Term Storage at 5°C.

Because of high diurnal water quality fluctuations in raw municipal wastewater, the use of proportional autosampling over a period of 24 h at municipal wastewater treatment plants (WWTPs) to evaluate carbon, nitrogen, and phosphorus removal has become a standard in many countries. Microbial removal or load estimation at municipal WWTPs, however, is still based on manually recovered grab samples. The goal of this study was to establish basic knowledge regarding the persistence of standard bacterial fecal indicators and Bacteroidetes genetic microbial source tracking markers in municipal wastewater in order to evaluate their suitability for automated sampling, as the potential lack of persistence is the main argument against such procedures. Raw and secondary treated wastewater of municipal origin from representative and well-characterized biological WWTPs without disinfection (organic carbon and nutrient removal) was investigated in microcosm experiments at 5 and 21°C with a total storage time of 32 h (including a 24-h autosampling component and an 8-h postsampling phase). Vegetative Escherichia coli and enterococci, as well as Clostridium perfringens spores, were selected as indicators for cultivation-based standard enumeration. Molecular analysis focused on total (AllBac) and human-associated genetic Bacteroidetes (BacHum-UCD, HF183 TaqMan) markers by using quantitative PCR, as well as 16S rRNA gene-based next-generation sequencing. The microbial parameters showed high persistence in both raw and treated wastewater at 5°C under the storage conditions used. Surprisingly, and in contrast to results obtained with treated wastewater, persistence of the microbial markers in raw wastewater was also high at 21°C. On the basis of our results, 24-h autosampling procedures with 5°C storage conditions can be recommended for the investigation of fecal indicators or Bacteroidetes genetic markers at municipal WWTPs. Such autosampling procedures will contribute to better understanding and monitoring of municipal WWTPs as sources of fecal pollution in water resources.

Considerations on methodological challenges for water footprint calculations.

We have investigated how different approaches for water footprint (WF) calculations lead to different results, taking sugar beet production and sugar refining as examples. To a large extent, results obtained from any WF calculation are reflective of the method used and the assumptions made. Real irrigation data for 59 European sugar beet growing areas showed inadequate estimation of irrigation water when a widely used simple approach was used. The method resulted in an overestimation of blue water and an underestimation of green water usage. Dependent on the chosen (available) water quality standard, the final grey WF can differ up to a factor of 10 and more. We conclude that further development and standardisation of the WF is needed to reach comparable and reliable results. A special focus should be on standardisation of the grey WF methodology based on receiving water quality standards.

Identification of relevant micropollutants in Austrian municipal wastewater and their behaviour during wastewater treatment.

The European Union has defined environmental quality standards (EQSs) for surface waters for priority substances and several other pollutants. Furthermore national EQSs for several chemicals are valid in Austria. The study investigated the occurrence of these compounds in municipal wastewater treatment plant (WWTP) effluents. In a first screening of 15 WWTPs relevant substances were identified, which subsequently were monitored in 9 WWTPs over 1 year (every 2 months). Out of 77 substances or groups of substances (including more than 90 substances) 13 were identified as potentially relevant in respect to water pollution and subjected to the monitoring, whereas most other compounds were detected in concentrations far below the respective EQS for surface waters and therefore not further considered. The preselected 13 compounds for monitoring were cadmium (Cd), nickel (Ni), copper (Cu), selenium (Se), zinc (Zn), diuron, polybrominated diphenyl ethers (PBDEs), di(ethyl-hydroxyl)phthalate (DEHP), tributyltin compounds (TBT), nonylphenoles (NP), adsorbable organic halogens (AOX) and the complexing agents ethylenediaminetetraacetic acid (EDTA) as well as nitrilotriacetic acid (NTA). In the effluents of WWTPs the concentrations of the priority substances Cd, NP, TBT and diuron frequently exceeded the respective EQS, whereas the concentrations for DEHP and Ni were below the respective EQS. The effluent concentrations for AOX, EDTA, NTA, Cu, Se and Zn frequently are in the range or above the Austrian EQS for surface waters. Besides diuron and EDTA all compounds are removed at least partially during wastewater treatment and for most substances the removal via the excess sludge is the major removal pathway. For the 13 compounds which were monitored in WWTP effluents population equivalent specific discharges were calculated. Since for many compounds no or only few information is available, these population equivalent specific discharges can be used to assess emissions from municipal WWTPs to surface waters as well as to make a first assessment of the impact of a discharge on surface waters chemical status. Comparing discharges and river pollution on a load basis, the influence of diffuse sources becomes obvious and therefore should also be taken into consideration in river management.

Foam formation on an Austrian-Hungarian lowland river: reasons, methods and solutions.

The occurrence of foam in a lowland river in Austria and shortly after the border with Hungary and the consequent protests from Hungarian inhabitants led to investigations concerning the reasons for foam formation. The aims of the study were (i) to specify objectively the scale of appearing of foam, (ii) to evaluate reasons for foam formation, and (iii) to develop abatement measures.

The combined approach--a challenge for border crossing water quality issues in Austria.

Is it sufficient to meet threshold values downstream of a discharge, even if this leaves no more space for future development? Is it simply bad luck for a downstream country, if threshold values are filled up at the border and there is no more space for additional emissions? If not: what are the criteria to distribute acceptable emissions between countries and regions? Who pays according to the "polluter pays" principle in a case, if several polluters contribute to the pollution, but the most cost-effective measures to reach the good status concern only some of the emitters/enterprises? There are little experiences with those and other related questions in Austria and many other EU-member states. This contribution intends to discuss these issues based on actual problems and would like to raise awareness for several of these unsolved questions.

Intelligent monitoring networks--transformation of data into information for water management.

The EU-WFD requires certain monitoring tasks, which yet cannot be fulfilled by automated monitoring devices. Nevertheless, the technical progress of recent years allows monitoring station designs, which enable long-term field application under reasonable maintenance demand. State-of-the-art monitoring stations allow the setup and operation of intelligent monitoring networks, which deliver quality proved and utilisable information to the end-user as opposed to a collection of time-series. Based on a full-scale example monitoring station design, long-term observations and possible ways of (automated) data interpretation are discussed.

Investigative monitoring in the context of detecting anthropogenic impact on an epipotamal river.

In the context of an investigative monitoring programme a monitoring system comprising of a water quality monitoring station and a camera station has been installed and operated for more than one year. The monitoring target was to investigate changes of water quality which can be related to a repeated occurrence of foam, observed at a river stretch downstream the monitoring station. The extent and frequency of foam buildup was recorded by means of the camera station. The analysis of the online data clearly showed that some of the measured parameters can be used as indicators for specific discharges, which from additional targeted investigations could be identified as contributors to the foaming problems. The continuous ammonium measurement could be used to detect nitrification problems of WWTPs discharging upstream of the monitoring station. By combining different data sources (emission data, operative and investigative monitoring data) additional information can be gained, which can be used for a comprehensive data assessment as well as a detailed system analysis.

Discussion of an environment quality standard based assessment procedure for permitting discharge.

The 'combined approach' as a requirement of the EC Water Framework Directive pools an emission-based approach with an approach based on environmental quality standards (EQS) to improve European water quality. The implementation of the EQS-based approach poses problems of defining a reference water discharge, defining a distance, where the EQS are obligatory and thus have to be controlled after point discharge, considering incomplete mixing. To elaborate a simple assessment procedure including the aspects mentioned above is the point of discussion in this paper. On the basis of easily available data and references from several European countries, recommendations for an Austrian assessment procedure are presented.

Monitoring of carbamazepine concentrations in wastewater and groundwater to quantify sewer leakage.

Monitoring of carbamazepine concentrations in wastewater and groundwater enables us to identify and quantify sewer exfiltration. The antiepileptic drug carbamazepine is hardly removed in wastewater treatment plants and not or just slightly attenuated during bank infiltration and subsoil flow. Concentrations in wastewater are generally 1000 times higher than the limit of quantification. In contrast to . many other wastewater tracers carbamazepine is discharged to the environment only via domestic wastewater. The results from this study carried out in Linz, Austria indicate an average exfiltration rate of 1%, expressed as percentage of the dry weather flow that is lost to the groundwater on the city-wide scale. This rate is lower than sewage losses reported in most other studies which attempted to quantify exfiltration on the basis of groundwater pollution. However, it was also possible to identify one area with significantly higher sewage losses. This method seems to be very suitable for the verification of leakage models used to assess sewer exfiltration on a regional scale.

Lessons learned from investigations on case study level for modelling of nutrient emissions in the Danube basin.

In the framework of the project daNUbs (Nutrient Management in the Danube Basin and its Impact on the Black Sea) the MONERIS emission model is used for the basin wide calculation of nutrient (nitrogen and phosphorus) emissions in the Danube Basin. The MONERIS model was developed and successfully applied for German river catchments. Based on investigations in selected test regions (case studies) the daNUbs approach is to check the applicability of the MONERIS emission model for the specific conditions of the Danube Basin in more detail than is possible with a basin wide application. Six case studies with areas of 400-3,500 km2 and several subcatchments have been selected in order to represent different conditions along the Danube Basin. In this study region intensive data collection and enhanced monitoring has been performed in order to raise the database significantly above the generally available data. Water balance as well as nutrient balance calculations have been performed with the MONERIS model as well as with other approaches. Results are compared to each other and to data from monitoring. Results up till now showed the applicability and sensitivity of the MONERIS approach in different conditions of the Danube Basin (e.g. emissions via groundwater). They indicated that the nitrogen retention in the catchments is well described with the MONERIS model.

Considerations on the influence of extreme events on the phosphorus transport from river catchments to the sea.

In this paper, results from rivers of different sizes in Romania, Hungary and Austria are presented. The paper shows the dynamics of extreme events and their contribution to the total P and suspended solids transported in these rivers. Special attention is paid to the influence of the size of the catchment and the event probability on the relative contribution of a single event to the total loads transported in the river. Further, the development of phosphorus loads along the Danube River at a flood event is shown. From the results it can be concluded that there is no immediate influence of high flow and flood events in upstream parts of the Basin on the transport of phosphorus from the catchment to the receiving Sea. Particle-bound phosphorus is mobilised from the catchment (through erosion) and the river bottom to a high extent at high flow events and transported at peak discharges to downstream, where retention by sedimentation of particles takes place. On the one hand this retention is a transport to flooded areas. In this case it can be considered as more or less long term retention. On the other hand sedimentation takes place in the riverbed, in case the tractive effort of the river is reduced. In this second case the P-pool in the sediments of the sedimentation area will be increased. If anaerobic conditions in the sediment appear, part of the phosphorus will be transformed to soluble ortho-phosphate and will continuously contribute to the phosphorus transport to the receiving sea. Part of the P-retained in the river sediment will be mobilised by resuspension at the next biggest high flow event. Altogether, these alternating processes of suspension, transport, export to flooded areas or sedimentation in the river bed with partly solution and partly resuspension at the next event decrease the share of the phosphorus transport during high flow events on the total loads transported in the more downstream parts of a catchments as compared to the more upstream parts. In the year of occurrence of an extreme flood event the P-transport of this year is dominated by the flood event. As an average over many years the contribution of high flow events to the total P-transport still may be between 7 and 20% in smaller catchments (around 1,000 km2). In a big catchment (e.g. river Danube) much smaller contributions of flood events on the total P-transport can be expected as an average over many years.

Nutrient emissions from diffuse and point sources into the River Danube and its main tributaries for the period of 1998-2000--results and problems.

Nutrient emissions by point and diffuse sources were estimated for 388 sub-catchments of the Danube river basin for the period 1998-2000 by means of the Model MONERIS. For nitrogen total emissions of 684 kt/a N were estimated for the Danube basin. 80% of these emissions were caused by diffuse sources (mainly groundwater, urban areas and tile drainage). For phosphorus the emission was 57 kt/a P, with a contribution of diffuse sources to this sum of 58%. The comparison of calculated and observed loads shows that the mean deviation for the investigated sub-catchments of the Danube river basin is 20% for dissolved inorganic nitrogen and 34% for phosphorus. The spatial resolution of the emission calculations allows the identification of regional hot spots and the derivation of specific regional measures to reduce the emissions into the Danube and consequently into the Western Black Sea.

Nitrogen fluxes on catchment scale: the influence of hydrological aspects.

In two catchment areas with altogether eight subcatchments characterising different site-specific situations the interaction between anthropogenic activities (e.g. agriculture, nutrition and waste water management), nitrogen emissions and in stream loads as well as concentrations were studied in detail. Groundwater is the most important pathway for nitrogen inputs into surface waters. Denitrification in the soil/subsurface/groundwater system controls the amount of this input to a high extent. Key factors influencing this process are organic carbon availability, geology, precipitation and groundwater recharge rates as well as residence time in groundwater. The MONERIS emission model is a useful tool to quantify these relationships on (sub-)catchment scale. Areas where concentrations in groundwater (e.g. nitrate) tend to be higher due to little dilution with water and might be problematic in respect to limit values for drinking water, are much less relevant in respect to the loads transported to river systems and receiving seas, than regions with high precipitation. In cases with high water availability mainly high loads transported downstream and finally to the receiving sea are a considerable problem. Within a region mainly areas close to river systems contribute to nitrogen discharges to the river system because of the short residence times of the groundwater from these areas and--related to this--a lower influence of denitrification in the groundwater.

Estimations of municipal point source pollution in the context of river basin management.

Integrated presentation of total emissions on catchment scale is prerequisite for many tasks in integrated management of point and diffuse sources of pollution. This paper will focus on emissions of nutrients from municipal point sources. Based on calculations of discharges of N, P from households into wastewater and on the detailed evaluation of data from 76 municipal wastewater treatments plants, this paper presents ranges of specific loads of inhabitants and population equivalents in the raw wastewater. In addition data of these treatment plants have been evaluated in respect of the treatment efficiency for nitrogen and phosphorus (average reduction rates) dependent on the design characteristic (with or without nitrification, denitrification or enhanced phosphorus removal). The results of the investigation show that the specific N and P loads from households in Austria lie within the range 1.6-2.0 g P/(inhabitant.d) and 11- 13 g N/(inhabitant.d). The specific contribution of industries to municipal wastewater varies between 0.3 and 2.0 gP/(pe.d) and 0 and 13 g N/(pe.d) with average values of 1.3 g P/(pe.d) and 6.5 g N/(population equivalent (pe)/d). As average values for municipal wastewater (contributions from household and industry) this leads to specific influent loads of 1.5 g P/(pe.d) and 8.8 g N/(pe.d). Average treatment efficiencies of treatment plants are for instance 50% nitrogen removal in treatment plants with nitrification and 80% in treatment plants with nitrification/denitrification. For phosphorus a removal of about 85% can be expected where the treatment plant was designed for enhanced phosphorus removal. Finally a method for load estimations based on standard values as mentioned above was tested for the estimation of emission from municipal point sources of selected regions.